Observation of Competitive Nonadiabatic Photodissociation Dynamics of H2S+ Cations

Luan, Zhiwen1; Fu, Yanlin2; Tan, Yuxin1; Wang, Yaling1; Shan, Baokun1; Li, Jie1; Zhou, Xiaoguo1; Chen, Wentao1; Liu, Lijie1,2; Fu, Bina2; Zhang, Dong H.2; Yang, Xueming2,3; Wang, Xingan1

2022-09-01

10.1021/acs.jpclett.2c01892

Journal of Physical Chemistry Letters   影响因子和分区

1948-7185

A comprehensive understanding of dissociation mechanisms is of fundamental importance in the photochemistry of small molecules. Here, we investigated the detailed photodissociation dynamics of H2S+ near 337 nm by using the velocity map ion imaging technique together with the theoretical characterizations by developing global full-dimensional potential energy surfaces (PESs). Rotational state resolved images were acquired for the S+(4S) + H2 product channel. Significant changes in product total kinetic energy release distributions and angular distributions have been observed within a small excitation photon energy range of 5 wavenumbers. Analysis based on the full-dimensional PESs reveals that two nonadiabatic pathways determined by the transition state connecting two minima on the 12A ' state are responsible for the dramatic variation of observed product distributions. The current study has directly witnessed the competitive photodissociation mechanisms controlled by a critical energy point on the PES, thereby providing in-depth insight into the nonadiabatic dynamics in photochemistry.

SCI ; EI

英语

NI论文

其他

National Key R&D Program of China[2016YFF0200500] ; National Natural Science Foundation of China["22125302","22173099","22288201","21873089"] ; LiaoNing Revitalization Talents Program[XLYC1907190]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Atomic, Molecular & Chemical

WOS:000847908300001

AMER CHEMICAL SOC

20223612699178

Kinetic energy ; Photodissociation ; Potential energy ; Quantum chemistry

Fluid Flow, General:631.1 ; Physical Chemistry:801.4 ; Classical Physics; Quantum Theory; Relativity:931

Web of Science

1.Univ Sci & Technol China, Dept Chem Phys, Hefei 230026, Peoples R China
2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China
3.Southern Univ Sci & Technol, Sch Sci, Dept Chem, Shenzhen 518055, Peoples R China

Luan, Zhiwen,Fu, Yanlin,Tan, Yuxin,et al. Observation of Competitive Nonadiabatic Photodissociation Dynamics of H2S+ Cations[J]. Journal of Physical Chemistry Letters,2022,13(34):8157-8162.

Luan, Zhiwen.,Fu, Yanlin.,Tan, Yuxin.,Wang, Yaling.,Shan, Baokun.,...&Wang, Xingan.(2022).Observation of Competitive Nonadiabatic Photodissociation Dynamics of H2S+ Cations.Journal of Physical Chemistry Letters,13(34),8157-8162.

Luan, Zhiwen,et al."Observation of Competitive Nonadiabatic Photodissociation Dynamics of H2S+ Cations".Journal of Physical Chemistry Letters 13.34(2022):8157-8162.